High quality graphene synthesized by atmospheric pressure CVD on copper foil

Graphene was synthesized at 1000 °C by Atmospheric Pressure Chemical Vapor Deposition on copper foil from methane diluted in argon and hydrogen. The influence of the main synthesis parameters was studied on 2 × 2 cm2 foils in order to obtain continuous monolayer graphene without crystalline defect. The uniformity, crystal quality and number of layers of graphene were analyzed by Raman spectroscopy and Scanning Electronic Microscopy. First, an increase of the annealing pre-treatment duration induced an increase of the average size of copper grains, leading to larger graphene flakes of higher crystallinity presenting a lower number of layers. Similar evolutions of graphene characteristics were observed when decreasing the methane concentration to 20 ppm, whereas an increase of run duration led to a loss of graphene quality and to a higher number of graphene layers, confirming that graphene formation is not self-limiting on copper. An optimum hydrogen/methane ratio was found, quite different from other results of the literature, probably due to differences in the copper pre-treatment step. Finally, an optimized three step process was developed to form monolayer continuous graphene of high quality, successfully transposed to 7 × 7 cm2 substrates after a reactor scale-up.